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Isómeros de enlace de nitrosilo: NO acoplamiento a N₂O en un sitio mononuclear

Subrata Kundu^1,2, Phan N Phu³, Pokhraj Ghosh¹

¹Department of Chemistry , Georgetown University , Box 571227-1227, Washington , D. C. 20057 , United States.

Journal of the American Chemical Society

|January 3, 2019

Resumen

Los investigadores detallaron un mecanismo molecular para reducir el óxido nítrico (NO) a óxido nitroso (N2O), un gas de efecto invernadero, utilizando complejos de níquel-nitrosilo. Este estudio aclara la formación de nitrosilos raros y las vías de producción de N2O.

Área de la Ciencia:

Química inorgánica
Catálisis
Química de los gases de efecto invernadero

Sus antecedentes:

La reducción del óxido nítrico (NO) a óxido nitroso (N2O), un potente gas de efecto invernadero, es crucial en varios procesos químicos y biológicos.
Los sitios monometálicos y los complejos metal-nitrosilo son intermediarios clave en la reducción del NO.
Los factores que rigen la formación de raros isómeros de nitrosilo de lado siguen siendo poco conocidos.

Objetivo del estudio:

Para elucidar la formación de isómeros de enlace níquel-nitrosilo.
Investigar el mecanismo de reducción del óxido nítrico (NO) a óxido nitroso (N2O) en un sitio de metal mononuclear.
Comprender el papel de las interacciones no covalentes en el control de la coordinación del ligando de nitrosilo.

Principales métodos:

Síntesis y caracterización de los complejos níquel-nitrosilo.
Ajuste controlado de las interacciones no covalentes utilizando cationes de potasio.
Análisis espectroscópico para identificar isómeros de enlace y productos intermedios.
Estudios mecánicos de la reducción de NO y la liberación de N2O.

Principales resultados:

Se sintetizó y caracterizó con éxito un par de isómeros de enlace níquel-nitrosilo.
Las interacciones no covalentes controladas influyeron en la formación de isómeros específicos de nitrosilo.
Se propuso un mecanismo molecular escalonado para la reducción de NO a N2O, que implica el acoplamiento radical y un intermediario cis-hiponitrito.
La densidad de espín centrada en N en las especies de metal-nitrosilo reducido facilita el acoplamiento radical con NO.

Conclusiones:

Este estudio proporciona un mecanismo molecular detallado para la formación de N2O a partir de la reducción de NO en un sitio mononuclear.
Los hallazgos ofrecen información sobre la formación de nitrosilos laterales raros y su papel en la catálisis.
La comprensión de esta vía puede informar las estrategias para controlar las emisiones de gases de efecto invernadero y los procesos biológicos relacionados.

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